期刊
ADVANCED FUNCTIONAL MATERIALS
卷 28, 期 45, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201804355
关键词
electrolysis; electrolyzer; Pourbaix diagram; stability; X-ray absorption spectroscopy
类别
资金
- Swiss National Science Foundation through its Ambizione Program
- CCEM through the project RENERG2
- Swiss Competence Center for Energy Research (SCCER) Heat & Electricity Storage through Innosuisse, Switzerland
- Paul Scherrer Institute
- NCCR Marvel through the project RENERG2
It is shown that producing PrBaCo2O5+delta and Ba0.5Sr0.5Co0.8Fe0.2O2+delta nanoparticle by a scalable synthesis method leads to high mass activities for the oxygen evolution reaction (OER) with outstanding improvements by 10x and 50x, respectively, compared to those prepared via the state-of-the-art synthesis method. Here, detailed comparisons at both laboratory and industrial scales show that Ba0.5Sr0.5Co0.8Fe0.2O2+delta appears to be the most active and stable perovskite catalyst under alkaline conditions, while PrBaCo2O5+delta reveals thermodynamic instability described by the density-functional theory based Pourbaix diagrams highlighting cation dissolution under OER conditions. Operando X-ray absorption spectroscopy is used in parallel to monitor electronic and structural changes of the catalysts during OER. The exceptional BSCF functional stability can be correlated to its thermodynamic meta-stability under OER conditions as highlighted by Pourbaix diagram analysis. BSCF is able to dynamically self-reconstruct its surface, leading to formation of Co-based oxy(hydroxide) layers while retaining its structural stability. Differently, PBCO demonstrates a high initial OER activity while it undergoes a degradation process considering its thermodynamic instability under OER conditions as anticipated by its Pourbaix diagram. Overall, this work demonstrates a synergetic approach of using both experimental and theoretical studies to understand the behavior of perovskite catalysts.
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